Apparatus for the manufacture of sulphuric anhydride



P. AUDIANNE APPARATUS FORTHEMANUFACTUREOF SULPHURIC ANHYDRIDE Flat] Padded Apr. 1923. UNITED STAT PAUL AUPIANN'E, OF PARIS,

FRANCE, ASSIGNOB TO ETABLISSENTS KUHLKANN, F

PARIS, FRANCE. a

arrana'rus ron rnn nnnurnc'runn or sunrnunrc Auniznnmn.

To all whom it It is known that the latter procem for- V manufacture consists incausing oxygen from of a catalyst the air to act upon sulphurous anhydride at a temperature of about 500, in the presence which is platinum, generally,'in an extremely divided state carried by an inert support such as pumice-stone, asbestos mixture, but, it has 7 in order to obtain a good-working, it is mor magnesium sulphate. Since the reaction between oxygen and sulphurous anhydride is an exothermic one, it is possible to dispense with a preliminary heating .of the'gaseo'us been ascertained that dispensable to have a uniform temperature in thewhole mass and a perfectly uniform distribution of the gas through the catalyst. The apparatus: hitherto employed for the manufacture of sulphuric anhydride by the contact method may .be divided into two classes.

In the first class the. contact mass consists of asbestos or other carrier, platinized to the extent of 8% or 10% .and requires for a given daily output of the apparatus, a relatively small bulk,

, of the second class which is particularly proportion of 1 used the prooessof rillo the contact mass contains only 0.2 to 0.4% of platinum and occupies a v t dealof space in the cubic meter per ton of daily ouiliput of. anhydride. o

' uniformity of temperature w with known appara us of this second" type which also have considerable advan tages,'the above stated conditions for eflicient working, namely perfect distribution .of the gas through the catalytic mass and entire mass, areinsufiiciently satisfied,

The apparatus according to; the-present invention while belonging to the second type, avoids this drawback by approximating the construction tus and' it consists essentially of a vert cal cylindrical chamber called cataly ser cha n Application and July 29,

whereas 111 apparatus throughout this of catalyst. of the type of a'ppara- 1920. 'Serial 1l'o.'399,714=.

her inside .which a plurality of vertical tubes open at both ends are provided. 'Contrary to what has hitherto been the practice, the catalytic mass is arranged between the tubes, the mixture of sulphurous anhydride and air coming" from below, enters and passes upwardly through the tubes and passes downwardly between said tubes through the catalytic mass.

This arrangement has the advantage of enabling a large volume of .the mass having a small percentage of catalyst to be used,'without belng compelled to have a large number of tubes, or tubes having a diameter that is too large to allow the desired thermal exchange to take place properly.

In order to obtain a perfect uniformity of temperature, provision is made for ensurmg' a constant speed of the-flow of gasup and down throughout the whole apparatus.

The mixture of sulphurous anhydride and .air entering the tubes is\ compelled by the the tubes catalyst, outside of the tubes, the. catalytic reaction takes place with the evolution heat.

The uniformity of the distributionof the gases throughout the mass continues to be assured by the provision of outlet orifices d1- rected outwards towards an annular collector around. the whole periphery of' the catalyzer. e

- It will be seen that the apparatus forms thus a substantially perfect heat, exchanger, the cold gases which travel in the'tubes 2 be-- ing heated by the hot gases which trayel between the tubes. Thecoldestgases which are admitted to the exchanger 14; around the .tubes, are heated by the hottest (exit) gases travelling through tubes 1Q. [Besides the relative parat'us, the 'aly'zer, the diameter, length and the andspacing of the tubes are so selected the temperature shall remain almost perthroughout the entire. mass fectly constant A. heating device may dimensions of the ap- I diameter and-length of the catnumber.

that

be added in'- ce 'known manner to the apparatus with a View toobtaining theexchange of heat which is r starting the apparatus before immediately necessary for the best working,

The mixture after starting the apparatus.

of sulphurous anhydride and airis caused way and the temperature inside the cataeachother, at their lower I the passage of the tubes,

, tion between the holes provided lyzer has been sufficiently raised. In the accompanying drawings, which illustrate by way of example one mode of carrying the invention into effect,

,Fig. 1 is a section in elevation of the whole apparatus and F ig. 2 shows at a larger scale the details of a helicoidal stopper inserted in the lower end of each of the tubes as will be hereinafter more particularly referred to.

The apparatus consists essentially of a Vertical cylindrical chamber 1 called catalyzer chamber inside which is arranged a plurality of vertical tubes 2, the upper ends of which are freely open whilst the lower ends thereof are provided with a helicoidal stopper 3 allowing the gases to enter the tubes after being mixed (see Fig. 2). The tubes are held in proper space relation with part by means of a'tube-sheet (made for example of iron) 4 provided with the number of holes which are necessary for the passage of thetubes. At

their u per part the tubes are held by means of a tuffe-sheet (preferably of iron) 5, whilst the intervals between the holesserving for are pierced with a large number of holes of a small diameter (say about 10 mm) The lower ends of the tubes 2 which go beyond the plate 4, are in communication with a pipe 6 connected with the lower conical part of the chamber 1. The space between the tubes is filled for part of its height, with the catalyst 7 The latter rests ona sheet-iron 8, which is pierced with 'a-large number of holes of small secfor the passage of the tubes 2.

The space between the-tubes, for the remaining-part of the height, is filled with an inert substance 9 divided into small grains,

and carried by a. sheet-iron 10 similar to the sheet-iron 8. The said sheet-iron 10 separates the mass 9 from an annular collector 11 the internal lateral walls of which are also provided with a plurality of holes 12 and the collector communicates with a second chamber 14, hereinafter more particularly referred to, by means of a pipe 18. A plurality of tubes 29 provided in the walls of the chamber 1 allow the temperature of the mass to be taken at various heights by means of py'rometers.

The diameter of the chamber 1 and consequently the number of thetubes 2 are a function of the power of the catalyst, but-the mensions so that the most dimensions of the tubes and their spacing are determined so as to produce with the minimum amount of metal, the maximum of of tube-sheets 16 and 17 the tubes are placed in communication at their upper part with the chamber 1 through the pipe 13 and at theirlower part with an exhaust pipe 18. The space between the tubes is in communication with an inlet pipe 19 at the lower part and with a pipe 20 connected to the pipe 6, at the upper part. A valve 21 allows the said communication to be established or interrupted. For a catalyser of a given power the exchanger 14 has determined diperfect exchange of heat possible will be obtained. The pipe 6 is continued below the valve 21 by a pipe 22 provided with a valve 23 and leading to a heating device 24. The latter is placed also in communication with the pipe 6 (at the beginning of the operation) through a pipe 25 provided with a valve 26. Lastly a pipe 27 provided with a valve 28 is arranged between the pipe 19 for the inlet of cold gases and the connecting pipe 20, the said pipe 27 allowing part of the cold gases to he directed towards the chamber 1 Without traversing the heat-exchanger 14.

The working of the apparatus is as follows:

' During the normal operation of the apparatus, the .valve 21 is open, the valves 23 and 26 are closed. The mixture of sulphurous chamber 1 and to the resistance produced by 3, and goes downthe'helicoidal stoppers wardly between the tubes-m contact with catalyst 7; thereaction then takes place.

the temperature rises and the gaseous sulphuric anhydride enters the collector 10.

The gas travelling upwardly through the tubes, is given a whirlingmotion in the tubes, by which the heat transfer from the filling material 9 and catalyzer material 7 is increased. This motion is imparted to the gases by the plugs 3. These plugs also aid in causing the incoming gases to spreadout more uniformly in the lower end of chamber 1, so that the flow of gases upwardly through all the tubes will be more uniform. If these were omitted, much more gas would pass up through the tubes directly over the pipe 6 than through those near the periphery of chamber 1. It will be tubes being heated by chamber 14 through the pipe 13, enters the tubes 15 and leaves the chamber 14 through the pipe 18. There is a farther exchange of I heat in '14, the hot gases coming down the tubes heating the cold gases which travel upwardly-around the said tubes. An excellent working and a very good efiiciency of the apparatus are obtained owing to the homogeneousness of the temperature, especially through the catalyzer mass. The adjustment of the temperature in the catalyzer chamber 1 is efi'ected (after the process is started) by opening. more or less the'valve 28 which allows a portion, more or less great, of the -cold gases to passdirectly from pipe 18 into the pipe 20, and thence into the catalyzer chamber 1.

For starting the apparatus, when no reaction has yet taken place, it is advisable to heat the gases in order to obtain a good starting. The operation is as follows: the valve 21 is closed, the valves 23 and 26 are open and the mixture of sul hurous anhydride and air traverses the lieating device 24 before entering the catalyzer chamber 1. As soon as the reaction has commenced, the heating device is placed out of the circuit by re-openingthe valve 21 and by closing the valves 23 and 26.

What I claim is:-

1. An apparatus for the, manufacture of sulphuric anhydride by. the contact method comprising incombination a chamber, a plurality of vertical tubesin the said chamber a catalyst placed between and around the said' tubes, means for distributing a mixture containing sulfurous anhydride and oxygen inside the said tubes, means for causing the said mixture to rise inside the said tubes, and to flow downwardly'through the catalyst, and means for'maintaining a substantially uniform temperature throughout the height" of the mass of catalyzer material. 2. An apparatus for the manufacture of sulphuric anhydride by the contact method, comprising incombination, a chamber the bottom of which is of conical shape, an inlet orifice for the gas mixture at the apex of the said conical bottom, a plurality of vertical tubes in the said chamber, helical plugs at the lower parts of the said tubes, a catalyst placed between the said tubes, outlet orifices for the gas mixture around the whole periphery of the lower part of the chamber, an annular collector in communiwardly for causing the mixture to inside-the said tubes and to flow downwardly through the catalyst, the diameter and the length of the chamber, the diameter, the length number and spacing of the tubes being adapted formaintaining a substantially constant temperature of gases throughout the depth of the contact mass.

3-.In an apparatus for making S0 by the oxidation of SO by a catalyst, the bination of a contact chamber having a gas inlet at its lower part such lower part also constituting a gas distributor, a series of vertical tubes leading upwardly from such gas distributor to near the top of said ber, such chamber being closed at its top, an inert filling material surrounding the lower parts of said tubes and filling the" surrounding the upper parts of said tubesv and filling the Spaces therebetween, and exit means for treated gases located near the lower end of. said chamber but above the gas distributor.

4. A method ofi oxidizing S0 by oxygen, which comprises introducing a gas mixture containing said constituents, into a distributing chamber, causing such gas ture to travel substantially uniformly in wardly as a number of separate am within the bulk of a large body of a catalytic material having a degree of activity substantially equal to that. of platinized asbestos carrying about 0.2 to 0.4% of platinum, such passage of gas being in heatconducting relationship with all portions of mixture containing said constituents, into a distributing chamber, causing such gas mixture to travel substantially uniformly upas anumber of separate within the bulk of a largcbody of a cata lyti'c material having a degree of activity substantially equal to that of platinized asbestos carrying about 0.2'to 0.4% of platinum, such passage of gas being in heat-conducting relationship with all portions of said mass of catalytic material but not in actual contact therewith, then passing the gases downwardly through and in actual cation with the said outlet orifices, meanS-ocontact with said mass of catalytic material while allowing a transfer of heat from the catalytic material into the upwardly flowing streams of gas mixture, and maintaining the entire body of catalytic material at sub- 5 stantially uniform temperature after the commencement of the process, and'thereafter passing the gases through a body of inert 7 material, and in contact therewith, while transferring heat from the said gases into the said streams of incoming gas.

In testimony whereof I have signed my name to this specification PAUL AUDIANNE. 

